Ultrafast nonlinear optical response of Ag nanoparticles embedded in mesoporous thin films

Highly dispersed silver nanoparticles embedded in mesoporous thin films (MTFs) have been synthesized by modification of the interior surface of mesoporous silica with ethylenediamine moieties, which provided the coordination sites for the Ag ions, and subsequent reduction under hydrogen atmosphere. TEM observations show the mesoporous parent films have effectively controlled the growth of the synthesized silver nanoparticles. The composite films had an ultrafast nonlinear response time, as fast as 200 fs, and a third-order nonlinear optical susceptibility of 0.94 × 10^?10 esu, which was enhanced by the local field enhancement effect that was present when the silver nanoparticles were embedded in the surrounding dielectric matrix. The origin of the ultrafast nonlinear response and the enhanced nonlinearity of the composite films are attributed to the intraband transition of the free electrons near the Fermi surface of the incorporated silver nanoparticles.